Systematic and Automated Development of Quantum Mechanically Derived Force Fields: The Challenging Case of Halogenated Hydrocarbons
| العنوان: | Systematic and Automated Development of Quantum Mechanically Derived Force Fields: The Challenging Case of Halogenated Hydrocarbons |
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| المؤلفون: | Marco Campetella, Paolo Roberto Livotto, Ivo Cacelli, Nicola De Mitri, Giacomo Prampolini |
| المصدر: | Journal of chemical theory and computation 12 (2016): 5525–5540. doi:10.1021/acs.jctc.6b00705 info:cnr-pdr/source/autori:Prampolini G.; Campetella M.; De Mitri N.; Livotto P.R.; Cacelli I./titolo:Systematic and Automated Development of Quantum Mechanically Derived Force Fields: The Challenging Case of Halogenated Hydrocarbons/doi:10.1021%2Facs.jctc.6b00705/rivista:Journal of chemical theory and computation/anno:2016/pagina_da:5525/pagina_a:5540/intervallo_pagine:5525–5540/volume:12 |
| بيانات النشر: | American Chemical Society (ACS), 2016. |
| سنة النشر: | 2016 |
| مصطلحات موضوعية: | Computer Science Applications, Physical and Theoretical Chemistry, 010304 chemical physics, first principle, Chemistry, Intermolecular force, force field parameters, halogenated hydrocarbons, 010402 general chemistry, 01 natural sciences, Force field (chemistry), 0104 chemical sciences, Computer Science Applications, Theoretical physics, 0103 physical sciences, A priori and a posteriori, Density functional theory, Statistical physics, Physical and Theoretical Chemistry, Quantum, a priori parametrization |
| الوصف: | A robust and automated protocol for the derivation of sound force field parameters, suitable for condensed-phase classical simulations, is here tested and validated on several halogenated hydrocarbons, a class of compounds for which standard force fields have often been reported to deliver rather inaccurate performances. The major strength of the proposed protocol is that all of the parameters are derived only from first principles because all of the information required is retrieved from quantum mechanical data, purposely computed for the investigated molecule. This a priori parametrization is carried out separately for the intra- and intermolecular contributions to the force fields, respectively exploiting the Joyce and Picky programs, previously developed in our group. To avoid high computational costs, all quantum mechanical calculations were performed exploiting the density functional theory. Because the choice of the functional is known to be crucial for the description of the intermolecular interactions, a specific procedure is proposed, which allows for a reliable benchmark of different functionals against higher-level data. The intramolecular and intermolecular contribution are eventually joined together, and the resulting quantum mechanically derived force field is thereafter employed in lengthy molecular dynamics simulations to compute several thermodynamic properties that characterize the resulting bulk phase. The accuracy of the proposed parametrization protocol is finally validated by comparing the computed macroscopic observables with the available experimental counterparts. It is found that, on average, the proposed approach is capable of yielding a consistent description of the investigated set, often outperforming the literature standard force fields, or at least delivering results of similar accuracy. |
| تدمد: | 1549-9626 1549-9618 |
| DOI: | 10.1021/acs.jctc.6b00705 |
| URL الوصول: | https://explore.openaire.eu/search/publication?articleId=doi_dedup___::708b027d8dc745f64975f17f5b007d9f https://doi.org/10.1021/acs.jctc.6b00705 |
| Rights: | OPEN |
| رقم الانضمام: | edsair.doi.dedup.....708b027d8dc745f64975f17f5b007d9f |
| قاعدة البيانات: | OpenAIRE |
| تدمد: | 15499626 15499618 |
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| DOI: | 10.1021/acs.jctc.6b00705 |